PAA

PAA
  • 文章类型: Journal Article
    氯化氪(KrCl*)准分子灯(222nm)被用作有前途的辐射源,可在水处理中驱动基于紫外线的高级氧化工艺(UV-AOP)。在这项研究中,UV222/过乙酸(PAA)工艺是一种新型的UV-AOPs,用于降解水中的新兴污染物(EC)。结果表明,UV222/PAA工艺对卡马西平(CBZ)具有优异的降解性能,45min内去除率达90.8%。值得注意的是,在相同UV剂量下,UV222/PAA工艺中CBZ的降解(90.8%)显著高于UV254/PAA工艺中CBZ的降解(15.1%)。UV222/PAA工艺表现出优异的每订单电能(EE/O)性能,同时减少与高能UV254/PAA工艺相关的资源消耗。淬火实验和电子顺磁共振(EPR)检测证实,HO•在反应中起主导作用。直接光解的贡献,HO•,和其他活性物种(RO和1O2)估计为5%,88%,7%,分别。此外,Cl-的影响,HCO3-,和腐殖酸(HA)对CBZ的降解停止了评价。相对低浓度的Cl-的存在,HCO3-,和HA可以抑制CBZ降解。UV222/PAA氧化过程还可以有效降解其他几种EC(即,碘海醇,磺胺甲恶唑,乙草胺,布洛芬),表明该工艺在污染物去除中的潜在应用。这些发现将推动UV222/PAA工艺的发展,并为其在水处理中的应用提供有价值的见解。
    Krypton chloride (KrCl*) excimer lamps (222 nm) are used as a promising irradiation source to drive ultraviolet-based advanced oxidation processes (UV-AOPs) in water treatment. In this study, the UV222/peracetic acid (PAA) process is implemented as a novel UV-AOPs for the degradation of emerging contaminants (ECs) in water. The results demonstrate that UV222/PAA process exhibits excellent degradation performance for carbamazepine (CBZ), with a removal rate of 90.8 % within 45 min. Notably, the degradation of CBZ in the UV222/PAA process (90.8 %) was significantly higher than that in the UV254/PAA process (15.1 %) at the same UV dose. The UV222/PAA process exhibits superior electrical energy per order (EE/O) performance while reducing resource consumption associated with the high-energy UV254/PAA process. Quenching experiments and electron paramagnetic resonance (EPR) detection confirm that HO• play a dominant role in the reaction. The contributions of direct photolysis, HO•, and other active species (RO• and 1O2) are estimated to be 5 %, 88 %, and 7 %, respectively. In addition, the effects of Cl-, HCO3-, and humic acid (HA) on the degradation of CBZ are evaluated. The presence of relatively low concentrations of Cl-, HCO3-, and HA can inhibit CBZ degradation. The UV222/PAA oxidation process could also effectively degrade several other ECs (i.e., iohexol, sulfamethoxazole, acetochlor, ibuprofen), indicating the potential application of this process in pollutant removal. These findings will propel the development of the UV222/PAA process and provide valuable insights for its application in water treatment.
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  • 文章类型: Journal Article
    铅(II)是重金属离子(HIs)的潜在致癌物。随着含铅产品包括铅合金产品的广泛应用,和新能源铅离子电池,铅污染已经成为一个棘手的问题。为了解决这样的困难,通过丙烯酸共聚合成了具有“弹簧”效应的新型超薄MoS2-乙烯基杂化膜(MVHM),研究了苯乙烯和二硫化钼(MoS2)及其对HIs的吸附作用。“弹簧”效应源于与MoS2连接的短聚丙烯酸(PAA)链向外扩散的趋势与MoS2(s-MoS2)的层间库仑力之间的相互作用,这扩大了MoS2层的间距,而不改变膜形成后的层数,将溶胀膜变为致密膜,并在厚度方向上将原始厚度从0.5cm减小到0.011mm。吸附实验表明,与其他五种金属离子Cu2+相比,这些MVHMs具有超强的吸附性能和对Pb2+的高选择性,Cd2+,Ni2+,Cr3+和Zn2+。尤其是,MVHM对Pb2+的吸附量可达2468mg/g,qe[Pb2+]/qe[Cu2+]的最大吸附比可达10.909。这些值比过去十年中报道的吸附剂获得的数据大得多。应用多种模子来评价离子基团的感化。证实了-COOH对HIs的吸附起关键作用,s-MoS2也有一定的贡献。相反,离子交换在吸附过程中只起次要作用。在这些金属离子中,Pb(II)的有效扩散系数(Deff)最大。因此,这些杂化膜是用于从含有各种离子的水中去除Pb2+的有前途的吸附剂。
    Lead(II) is a potential carcinogen of heavy-metal ions (HIs). With the wide application of Pb-bearing products including lead alloy products, and new-energy lead-ion batteries, lead pollution has become a tricky problem. To solve such a difficulty, novel ultrathin MoS2-vinyl hybrid membranes (MVHMs) with a \"spring\" effect were synthesized via co-polymerization of acrylic acid, styrene and molybdenum disulfide (MoS2) and their adsorptions for HIs were explored. The \"spring\" effect derived from the interaction between the tendency of the short polyacrylic acid (PAA) chain connected with MoS2 to spread outward and the coulomb force between layers from MoS2 (s-MoS2), which enlarge the spacing of MoS2 layers without changing the number of layers after membrane formation, which changes the swelling membrane to a dense membrane and reduces the original thickness from 0.5 cm to 0.011 mm in the thickness direction. The adsorption experiment revealed that these MVHMs had super adsorption performance and high selectivity for Pb2+ by comparison with other five metal ions: Cu2+, Cd2+, Ni2+, Cr3+ and Zn2+. Especially, the adsorption quantity of MVHMs for Pb2+ could approach 2468 mg/g and the maximum adsorption ratio of qe[Pb2+]/qe[Cu2+] can reach 10.909. These values were much larger than the data obtained with the adsorbents reported in the last decade. A variety of models are applied to evaluate the effect of ionic groups. It was confirmed that -COOH plays a key role in adsorption of HIs and s-MoS2 also has a certain contribution. Conversely, ion exchange plays only a minor role during the period of adsorption process. Effective diffusion coefficient (Deff) of Pb(II) had the largest values among these metal ions. Hence, these hybrid membranes are promising adsorbents for the removal of Pb2+ from water containing various ions.
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  • 文章类型: Journal Article
    实现对人体活动的稳定、实时监测,在木质素磺酸盐(LS)和Al3存在的情况下,使用聚丙烯酸(PAA)和羧甲基瓜尔胶(CMGG)制造了新型水凝胶,作为可穿戴且柔性的应变或压力传感器。基于金属配位键的共存,该系统中的氢键和离子相互作用,所获得的水凝胶表现出理想的机械性能和良好的自恢复能力。水凝胶表现出良好的自粘附行为和超高的拉伸灵敏度(应变系数(GF)=24.30),因此,它们可以精确检测人体关节的运动,如肘部,手腕,手指弯曲以及微小的运动和外部刺激,如吞咽,微笑,皱眉,脉搏,说话,写作,甚至不同液滴的下落。此外,30h后,水凝胶显示出优异的自修复能力,愈合效率高达100%。最重要的是,愈合的水凝胶可以执行与以前相同的传感性能。基于这些显著特征,这种水凝胶代表了长期和稳定的健康监测应用可穿戴和柔性传感器的巨大潜力。
    To realize on stable and real-time monitoring of human activities, novel hydrogels using polyacrylic acid (PAA) and carboxymethyl guar gum (CMGG) were fabricated as wearable and flexible strain or pressure sensors in the presence of lignosulfonate (LS) and Al3+. Based on the co-existence of metal coordination bonds, hydrogen bonds and ionic interaction in this system, the obtained hydrogels exhibited desirable mechanical properties with good self-recovery ability. The hydrogels displayed good self-adhesion behavior and an ultra-high tensile sensitivity (gauge factor (GF) = 24.30), therefore, they could precisely detect human joints movements such as elbow, wrist, and finger bending as well as tiny movements and external stimuli such as swallowing, smile, frown, pulse, speaking, writing, and even the falling of different liquid drops. Additionally, the hydrogels showed excellent self-healing ability with the healing efficiency as high as 100 % after 30 h. Most importantly, the healed hydrogel could perform the same sensing performance as before. Based on these distinguished characteristics, this hydrogel represents great potentials in wearable and flexible sensors for long-term and stable health monitoring application.
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  • 文章类型: Journal Article
    Nanorana属包含三个亚属,即Nanorana,Paa,还有Chaparana,目前,在Nanorana(Nanorana)中,科学已知有四个物种。在这项研究中,我们描述了一个属于云南西北部Nanorana亚属的新物种,中国。系统发育,新物种,Nanoranalaojunshanensissp。11月。,是N.pleskei和N.ventripunctata进化枝的妹妹。形态学上,新物种可以通过以下特征的组合与已知的同源物区分开来:目前的鼓室,手指I和II相等,身体尺寸小,四肢的黄色腹面,不同的vomerine牙齿,关节下结节,头部宽度大于头部长度,细长的鼓室上褶皱,背外侧褶皱缺失,成年男性手指I和II上存在的新刺,不存在声囊,并在胸部配对棕色的刺。此外,我们建议将Allopaa属移至Nanorana(Chaparana),并认为N.arunachalensis既不是Odorrana物种,也不是Dicroglossinae亚科(因此Nanorana)的成员,但可能代表与Ingerana密切相关或属于Ingerana的独特属,等待更多数据。此外,我们认为Nanoranaminica值得一个独立的亚属,我们建议指派N.Arnoldi,N.blanfordii,大头蛇,波卢尼尼,N.Rarica,N.rostati,N.Vicina,N.xuelinensis,和赵尔米进入Paa亚属,并放置康仙草,N.Phrynoides,和Chaparana亚属的四川N.
    The genus Nanorana contains three subgenera, namely Nanorana, Paa, and Chaparana, and currently, there are four species known to science in Nanorana (Nanorana). In this study, we describe a new species belonging to the subgenus Nanorana from northwestern Yunnan, China. Phylogenetically, the new species, Nanorana laojunshanensissp. nov., is the sister to the clade of N. pleskei and N. ventripunctata. Morphologically, the new species can be distinguished from known congeners by the combination of following characters: present tympanum, equal fingers I and II, small body size, yellow ventral surface of limbs, distinct vomerine teeth, indistinct subarticular tubercles, head width greater than head length, slender supratympanic fold, absent dorsolateral fold, nuptial spines present on fingers I and II in adult males, absent vocal sac, and paired brown spines on the chest. Moreover, we suggest moving the genus Allopaa into Nanorana (Chaparana) and consider that N. arunachalensis is neither an Odorrana species nor a member of the subfamily Dicroglossinae (therefore Nanorana), but probably represents a distinct genus closely related to Ingerana or belongs to Ingerana, pending more data. Additionally, we consider that Nanorana minica deserves the rank of an independent subgenus, and we suggest assigning N. arnoldi, N. blanfordii, N. ercepeae, N. polunini, N. rarica, N. rostandi, N. vicina, N. xuelinensis, and N. zhaoermii into the subgenus Paa and placing N. kangxianensis, N. phrynoides, and N. sichuanensis in the subgenus Chaparana.
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  • 文章类型: Journal Article
    消毒对于游泳池水(SPW)质量至关重要。过氧乙酸(PAA)因其优点(例如较少形成受调节的DBPs)而引起了人们对水消毒的关注。由于复杂的水基质源于游泳者的体液负荷和较长的停留时间,因此很难在游泳池中阐明消毒剂的持久性动力学。在这项研究中,PAA的持久性动力学在SPW中以游离氯为基准进行了研究,使用台架实验和模型模拟。建立了动力学模型来模拟PAA和氯的持久性。PAA的稳定性对游泳者负荷的敏感性低于氯。平均游泳者负荷事件使PAA的表观衰减速率常数降低了66%,随着温度升高而减弱的现象。来自游泳者的L-组氨酸和柠檬酸被确定为主要的阻滞因素。相比之下,游泳者装载事件瞬间消耗了70-75%的残余游离氯。在3天累积消毒模式下,所需的PAA总剂量比氯低97%。温度与消毒剂腐烂率呈正相关,PAA比氯更敏感。这些结果揭示了游泳池环境中PAA的持久性动力学及其影响因素。
    Disinfection is essential to swimming pool water (SPW) quality. Peracetic acid (PAA) has attracted attention for water disinfection for advantages such as less formation of regulated DBPs. Persistence kinetics of disinfectants is difficult to elucidate in pools because of the complex water matrix stemming from body fluid loadings from swimmers and long residence times. In this research, the persistence kinetics of PAA was investigated in SPW benchmarked against free chlorine, use bench-scale experiments and model simulation. Kinetics models were developed to simulate the persistence of PAA and chlorine. The stability of PAA was less sensitive to swimmer loadings than chlorine. An average swimmer loading event reduced the apparent decay rate constant of PAA by 66 %, a phenomenon that diminished with increasing temperatures. L-histidine and citric acid from swimmers were identified as main retardation contributors. By contrast, a swimmer loading event instantaneously consumed 70-75 % of the residual free chlorine. The required total dose of PAA was 97 % less than chlorine under the 3-days cumulative disinfection mode. Temperature was positively correlated with disinfectant decay rate, with PAA being more sensitive than chlorine. These results shed light on the persistence kinetics of PAA and its influential factors in swimming pool settings.
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  • 文章类型: Journal Article
    在无金属催化剂上基于过乙酸的高级氧化工艺(PAA-AOPs)已成为去除水污染物的迷人策略。然而,所涉及的反应性物种及其相应的活性位点是模糊的。在这里,使用碳纳米管(CNT)作为模型碳催化剂,我们证明了,在中性条件下,CNT-PAA*络合物是通过电子转移过程(ETP)氧化酚类化合物的主要反应性物种,而表面结合的羟基自由基(·OHsurface)在猝灭和电化学测试以及拉曼光谱的基础上起着次要作用。更重要的是,实验和密度泛函理论(DFT)计算结果共同证明,ETP的活性位点是CNT本体上的sp2杂化碳,虽然自由基生成是位于边缘的羟基(C-OH),这降低了CNT-PAA*复合物中裂解O-O键的能垒。我们从CNT/PAA系统中的表观动力学常数进一步辨别了不同污染物的氧化动力学常数(koxid)。酚类化合物的lnkoxid与半波电位之间的显着负线性相关表明,具有较低的单电子氧化电位的污染物(即,更强的给电子能力)更容易被氧化。总的来说,这项研究审查了混合自由基和非自由基机制和相应的活性位点的CNT/PAA系统,提供对PAA-AOPs的应用和ETP在新兴有机污染物修复中的发展的见解。
    Peracetic-acid-based advanced oxidation processes (PAA-AOPs) on metal-free catalysts have emerged as charming strategies for water contaminant removal. However, the involved reactive species and their corresponding active sites are ambiguous. Herein, using carbon nanotube (CNT) as a model carbocatalyst, we demonstrated that, under neutral conditions, the CNT-PAA* complex was the dominant reactive species to oxidize phenolic compounds via electron-transfer process (ETP), whereas the surface-bound hydroxyl radicals (·OHsurface) played a minor role on the basis of quenching and electrochemical tests as well as Raman spectroscopy. More importantly, the experimental and density functional theory (DFT) calculation results collaboratively proved that the active site for ETP was the sp2-hybridized carbon on the CNT bulk, while that for radical generation was the edge-located hydroxyl group (C-OH), which lowered the energy barrier for cleaving the O-O bond in CNT-PAA* complex. We further discerned the oxidation kinetic constants (koxid) of different pollutants from the apparent kinetic constants in CNT/PAA system. The significant negative linear correlation between lnkoxid and half-wave potential of phenolic compounds suggests that the pollutants with a lower one-electron oxidation potential (i.e., stronger electron-donating ability) are more easily oxidized. Overall, this study scrutinizes the hybrid radical and non-radical mechanism and the corresponding active sites of the CNT/PAA system, providing insights into the application of PAA-AOPs and the development of ETP in the remediation of emerging organic pollutants.
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  • 文章类型: Journal Article
    硅基阳极的应用价值尚未完全实现,因为其体积膨胀率为300%,电子导电性差。在目前的研究中,提出了一种介孔Si/C(MP-Si/C)复合材料,其纳米初级粒子为30-50nm,孔径为20-40nm,表现出优异的锂储存性能。首先,应用聚丙烯酸(PAA)来实现原位碳涂层,并抑制在stöber反应中由原硅酸四乙酯(TEOS)产生的SiO2的颗粒生长。其次,引入Mg气体以通过气割效应产生具有介孔和三维碳网络的纳米级Si。在2A/g和4A/g的情况下,400次循环后的容量为671mAh/g,500次循环后的容量为593mAh/g,循环稳定性和倍率性能均显着增强。分别,这与碳源PAA的选择及其相应的碳涂层和Mg还原效果高度相关。此外,这种方法绕过了昂贵的纳米硅的使用,这为硅基阳极的商业化提供了灵感。
    The application value of silicon-based anodes has not been fully realized due to the ∼ 300% volume expansion and poor electronic conductivity. In present study, mesoporous Si/C (MP-Si/C) composite with nanosized primary particles of 30-50 nm and pore diameter of 20-40 nm was proposed, which displays superior Li storage properties. Firstly, Polyacrylic acid (PAA) was applied to fulfill in-situ carbon coating and inhibit the particle growth of SiO2 generated from tetraethyl orthosilicate (TEOS) in stöber reaction. Secondly, Mg gas was introduced to create nano-sized Si with meso-pores and three-dimensional carbon network via the gas-cutting effect. The cycling stability and rate capability were both significantly enhanced with capacity of 671 mAh/g after 400 cycles and 593 mAh/g after 500 cycles at 2 A/g and 4 A/g, respectively, which was highly relevant to the selection of carbon source PAA and its corresponding carbon coating and Mg reduction effect. Moreover, this method bypasses the use of costly nano-silicon, which provides inspiration for the commercialization of silicon-based anodes.
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  • 文章类型: Journal Article
    In this study, we fabricated a composite polymer anion exchange membrane (AEM) with a sandwich structure. This prepared AEM demonstrated high ionic conductivity (0.25 Scm-1), excellent alkali resistance (8 M KOH), and good mechanical properties (tensile strength of 0.455 MPa and elongation at break of 82.13%). Here, degrease cotton (DC) treated with LiOH/urea aqueous solution was used and immersed into a coagulation bath to form a film. This film was immersed in acrylic acid (AA) monomers, and in-suit polymerization was carried out in the presence of KOH and an initiator. Finally, a composite polymer membrane with sandwich structure was achieved, in which the upper and bottom layers were mainly composed of polymerized AA (PAA) while the central layer was mainly composed of DC derived film. The central layer acted as a skeleton to improve the mechanical properties and alkali resistance. The top and bottom layers (PAA-rich layers) acted as OH- ion transport carriers, making basic cations migrate along the main chain of PAA. This newly developed composite membrane showed increased tensile strength and an elongation at break of 2.7 and 1.5 times, respectively, when compared to a control PAA/KOH AEM film. Furthermore, an electrochemical stability window of 2.0 V was measured via the cyclic voltammetry curve test, showing a wide electrochemical window and promising application in Zn-Air batteries.
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  • 文章类型: Journal Article
    To develop highly efficient T1/T2 magnetic resonance imaging (MRI) contrast agents (CAs), Gd/Y hydroxide nanosheets were synthesized by a simple exfoliation method from layer compounds using sodium polyacrylate (PAA) as a dispersant and stabilizer. Transmission electron microscopy (TEM) and atomic force microscopy (AFM) results revealed the excellent performance of monolayer nanosheets with thicknesses of up to 1.5 nm. The MRI results of the T1 and T2 relaxation times showed that all of the Gd/Y hydroxide nanosheets have high longitudinal and transverse relaxivities (r1 and r2). In particular, the 10% Gd-LRH nanosheets exhibited excellent MRI performance (r1 = 103 mM-1 s-1, r2 = 372 mM-1 s-1), which is rarely reported. Based on the relationship between the structure of 10% Gd-LRH nanosheets and their MRI performances, and the highly efficient MRI of spaced Gd atoms in the nanosheets, a special model to explain the outstanding MRI performance of the 10% Gd-LRH nanosheets is suggested. The cytotoxicity assessment of the 10% Gd-LRH nanosheets, evaluated by CCK-8 assays on HeLa cells, indicated no significant cytotoxicity. This study presents a significant advancement in 2D nanomaterial MRI CA research, with Gd-doped nanosheets positioned as highly efficient T1/T2 MRI CA candidates.
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  • 文章类型: Journal Article
    提供完整的双网络(样本缩写。:DN)水凝胶,聚(2-丙烯酰胺基-2-甲基丙磺酸)的两步交联反应(即,PAMPS首先网络),然后是聚(丙烯酸)(即,PAA第二网络)在交联剂存在下进行(N,N'-亚甲基双丙烯酰胺(MBAA)。类似于两步过程,不同含量的2,2,6,6-四甲基-1-哌啶基氧基(TEMPO)氧化纤维素纳米纤维(TOCN:1、2和3wt。%)最初分散在第一网络溶液中,然后交联。随后将含TOCN的PAMPS第一网络浸泡在AA和交联剂中并进行第二网络交联反应(对于DN样品,TOCN缩写为T)。作为第三步,然后用不同浓度的FeCl3(aq)溶液(5、50、100和200mM)处理各种(T-)DN水凝胶。通过将三价铁离子掺入(T-)DN水凝胶中,特别是,有三个目的:(i)通过离子键合增强(T-)DN水凝胶,(ii)显着赋予水凝胶的离子电导率,和(iii)用作第四步骤的催化剂,以进行吡咯的原位化学氧化聚合,以提供含聚吡咯的(样品摘要。:Py)水凝胶[即,(T-)Py-DN样品]。PAMPS的特征官能团,PAA,和Py经FT-IR确证。通过低温扫描电子显微镜(cryo-SEM)观察到均匀的微观结构。这些结果表明,通过四步法获得了T-Py-DN水凝胶的均匀复合材料。根据热重分析(TGA),所有干燥样品均显示出相似的热降解行为。T2-Py5-DN样本(即,含有2wt。%TOCN用5mMFeCl3(aq)处理)显示出最佳的拉伸强度和断裂性能应变(即,σTb=450kPa和εTb=106%)。用相同的构图,获得3.34×10-3S/cm的高电导率。坚韧的T2-Py5-DN水凝胶在50-100-0%的几个“拉伸和释放”循环中显示出良好的导电可逆性,展示了生物电子或生物材料应用的有前途的候选者。
    To afford an intact double network (sample abbr.: DN) hydrogel, two-step crosslinking reactions of poly(2-acrylamido-2-methylpropanesulfonic acid) (i.e., PAMPS first network) and then poly(acrylic acid) (i.e., PAA second network) were conducted both in the presence of crosslinker (N,N\'-methylenebisacrylamide (MBAA)). Similar to the two-step processes, different contents of 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) oxidized cellulose nanofibers (TOCN: 1, 2, and 3 wt.%) were initially dispersed in the first network solutions and then crosslinked. The TOCN-containing PAMPS first networks subsequently soaked in AA and crosslinker and conducted the second network crosslinking reactions (TOCN was then abbreviated as T for DN samples). As the third step, various (T-)DN hydrogels were then treated with different concentrations of FeCl3(aq) solutions (5, 50, 100, and 200 mM). Through incorporations of ferric ions into (T-)DN hydrogels, notably, three purposes are targeted: (i) strengthen the (T-)DN hydrogels through ionic bonding, (ii) significantly render ionic conductivity of hydrogels, and (iii) serve as a catalyst for the forth step to proceed with in situ chemical oxidative polymerizations of pyrroles to afford polypyrrole-containing (sample abbr.: Py) hydrogels [i.e., (T-)Py-DN samples]. The characteristic functional groups of PAMPS, PAA, and Py were confirmed by FT-IR. Uniform microstructures were observed by cryo scanning electron microscopy (cryo-SEM). These results indicated that homogeneous composites of T-Py-DN hydrogels were obtained through the four-step process. All dry samples showed similar thermal degradation behaviors from the thermogravimetric analysis (TGA). The T2-Py5-DN sample (i.e., containing 2 wt.% TOCN with 5 mM FeCl3(aq) treatment) showed the best tensile strength and strain at breaking properties (i.e., σTb = 450 kPa and εTb = 106%). With the same compositions, a high conductivity of 3.34 × 10-3 S/cm was acquired. The tough T2-Py5-DN hydrogel displayed good conductive reversibility during several \"stretching-and-releasing\" cycles of 50-100-0%, demonstrating a promising candidate for bioelectronic or biomaterial applications.
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